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A J Nozik

Publications and source records attributed to A J Nozik.

4 recordsLinked to original sources

Multiexciton generation by a single photon in nanocrystals.

We have theoretically shown that efficient generation of multi-electron-hole pairs by a single photon observed recently in semiconductor nanocrystals1-4 is caused by breaking the single electron approximation for carriers with kinetic energy above the effective energy gap. Due to strong Coulomb interaction, these states form a coherent superposition with charged excitons of the same energy. This concept allows us to define the conditions for dominant two-exciton generations by a single photon: the thermalization rate of a single exciton, initiated by light, should be lower than both the two-exciton state thermalization rate and the rate of Coulomb coupling between single and two exciton states. Possible experimental manifestations of our model are discussed.

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Exciton multiplication and relaxation dynamics in quantum dots: applications to ultrahigh-efficiency solar photon conversion.

Huge amounts of carbon-free energy will be required during the coming decades in order to stabilize atmospheric CO2 to acceptable levels. Solar energy is the largest source of non-carbonaceous energy and can be used to produce both electricity and fuel. However, the ratio of the areal cost to the conversion efficiency for devices converting solar photons to electricity or fuel must be reduced by at least 1 order of magnitude from the present values; this requires large increases in the cell efficiency and large reductions in the cost per unit area. We have shown how semiconductor quantum dots may greatly increase photon conversion efficiencies by producing multiple excitons from a single photon. This is possible because quantization of energy levels in quantum dots slows the cooling of hot excitons, promotes multiple exciton generation, and lowers the photon energy threshold for this process. Quantum yields of 300% for exciton formation in PbSe quantum dots have been reported at photon energies 3.8 times the HOMO-LUMO transition energy, indicating the formation of three excitons/photon for all photoexcited quantum dots. Similar high quantum yields have also been reported for PbS quantum dots. A new model for this effect that is based on a coherent superposition of multiple excitonic states has been proposed.

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Electron and hole transfer from indium phosphide quantum dots.

Electron- and hole-transfer reactions are studied in colloidal InP quantum dots (QDs). Photoluminescence quenching and time-resolved transient absorption (TA) measurements are utilized to examine hole transfer from photoexcited InP QDs to the hole acceptor N,N,N',N'-tetramethyl-p-phenylenediamine (TMPD) and electron transfer to nanocrystalline titanium dioxide (TiO2) films. Core-confined holes are effectively quenched by TMPD, resulting in a new approximately 4-ps component in the TA decay. It is found that electron transfer to TiO2 is primarily mediated through surface-localized states on the InP QDs.

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Spectroscopy and hot electron relaxation dynamics in semiconductor quantum wells and quantum dots.

Photoexcitation of a semiconductor with photons above the semiconductor band gap creates electrons and holes that are out of equilibrium. The rates at which the photogenerated charge carriers return to equilibrium via thermalization through carrier scattering, cooling by phonon emission, and radiative and nonradiative recombination are important issues. The relaxation processes can be greatly affected by quantization effects that arise when the carriers are confined to regions of space that are small compared with their deBroglie wavelength or the Bohr radius of bulk excitons. The effects of size quantization in semiconductor quantum wells (carrier confinement in one dimension) and quantum dots (carrier confinement in three dimensions) on the respective carrier relaxation processes are reviewed, with emphasis on electron cooling dynamics. The implications of these effects for applications involving radiant energy conversion are also discussed.

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